Crystal symmetry breaking and vacancies in colloidal lead chalcogenide quantum dots

Nature Materials

Volumn 15, Issue 9, 2016, Pages 987-994

  Bertolotti, Federica ^a   Dirin, Dmitry N ^b,c   Ibáñez, Maria ^b,c   Krumeich, Frank ^b   Cervellino, Antonio ^d   Frison, Ruggero ^e,f   Voznyy, Oleksandr ^g   Sargent, Edward H ^g   Kovalenko, Maksym V ^b,c   Guagliardi, Antonietta ^f   Masciocchi, Norberto ^a  

^a UNIVERSITY OF INSUBRIA   (Italy)

^b ETH ZURICH   (Switzerland)

^c SWISS FEDERAL LABORATORIES FOR MATERIALS SCIENCE AND TECHNOLOGY   (Switzerland)

^d PAUL SCHERRER INSTITUTE   (Switzerland)

^e UNIVERSITY OF ZURICH   (Switzerland)

^f CNR   (Italy)

^g UNIVERSITY OF TORONTO   (Canada)

Author keywords

[No Author keywords available]

Indexed keywords

CHALCOGENIDES; CRYSTAL ATOMIC STRUCTURE; CRYSTAL SYMMETRY; DENSITY FUNCTIONAL THEORY; LATTICE THEORY; LEAD; LEAD COMPOUNDS; LIGANDS; NANOCRYSTALS; OPTOELECTRONIC DEVICES; STRAIN; TENSILE STRAIN; X RAY SCATTERING;

BUILDING BLOCKES; LATTICE DISTORTIONS; LEAD CHALCOGENIDES; LOW-COST SOLUTION; ORIENTED ATTACHMENT; ROCK SALT STRUCTURES; STRUCTURAL DISTORTIONS; SYMMETRY-BREAKING;

SEMICONDUCTOR QUANTUM DOTS;

EID: 84974691369     PISSN: 14761122     EISSN: 14764660     Source Type: Journal    
DOI: 10.1038/nmat4661     Document Type: Article

References (34)

1. Kovalenko, M. V., et al. Prospects of nanoscience with nanocrystals. ACS Nano 9, 1012-1057 (2015).
2. Kovalenko, M. V., Scheele, M. & Talapin, D. V. Colloidal nanocrystals with molecular metal chalcogenide surface ligands. Science 324, 1417-1420 (2009).
3. Ibanez, M., et al. Electron doping in bottom-up engineered thermoelectric nanomaterials through HCl-mediated ligand displacement. J. Am. Chem. Soc. 137, 4046-4049 (2015).
4. Zhang, J., Gao, J., Miller, E. M., Luther, J. M. & Beard, M. C. High photocurrent PbSe solar cells with thin active layers. ACS Nano 8, 614-622 (2014).
5. Lan, X., Masala, S. & Sargent, E. H. Charge-extraction strategies for colloidal quantum dot photovoltaics. Nature Mater. 13, 233-240 (2014).
6. Zagorac, D., Doll, K., Schon, J. C. & Jansen, M. Sterically active electron pairs in lead sulfide? An investigation of the electronic and vibrational properties of PbS in the transition region between the rock salt and the -GeTe-type modifications. Chem. Eur. J. 108, 10929-10936 (2012).
7. Bozin, E. S., et al. Entropically stabilized local dipole formation in lead chalcogenides. Science 330, 1660-1663 (2010).
8. Kastbjerg, S., et al. Direct evidence of cation disorder in thermoelectric lead chalcogenides PbTe and PbS. Adv. Funct. Mater. 23, 5477-5483 (2013).
9. Moreels, I., et al. Size-tunable, bright, and stable PbS quantum dots: a surface chemistry study. ACS Nano 5, 2004-2012 (2011).
10. Moreels, I., Fritzinger, B., Martins, J. C. & Hens, Z. Surface chemistry of colloidal PbSe nanocrystals. J. Am. Chem. Soc. 130, 1581-1586 (2008).
11. Zherebetsky, D., et al. Hydroxylation of the surface of PbS nanocrystals passivated with oleic acid. Science 344, 1380-1383 (2014).
12. Anderson, N. C., Hendricks, M. P., Choi, J. J. & Owen, J. S. Ligand exchange and the stoichiometry of metal chalcogenide nanocrystals: spectroscopic observation of facile metal-carboxylate displacement and binding. J. Am. Chem. Soc. 135, 18536-18548 (2013).
13. Kim, D., Kim, D.-H., Lee, J.-H. & Grossman, J. C. Impact of stoichiometry on the electronic structure of PbS quantum dots. Phys. Rev. Lett. 110, 196802 (2013).
14. Cervellino, A., Frison, R., Bertolotti, F. & Guagliardi, A. DEBUSSY 2.0 the new release of a Debye user system for nanocrystalline and/or disordered materials. J. Appl. Crystallogr. 48, 2026-2032 (2015).
15. Chattopadhyay, T., Boucherlet, J. X. & von Schnering, H. G. Neutron diffraction study on the structural phase transition in GeTe. J. Phys. C 20, 1431-1440 (1987).
16. Berger, R., et al. Surface stress in the self-assembly of alkanethiols on gold. Science 276, 2021-2024 (1997).
17. Cho, K. S., Talapin, D. V., Gaschler, W. & Murray, C. B. Designing PbSe nanowires and nanorings through oriented attachment of nanoparticles. J. Am. Chem. Soc. 127, 7140-7147 (2005).
18. Klokkenburg, M., et al. Dipolar structures in colloidal dispersions of PbSe and CdSe quantum dots. Nano Lett. 7, 2931-2936 (2007).
19. Lee, S. M., Jun, Y.W., Cho, S. N. & Cheon, J. Single-crystalline star-shaped nanocrystals and their evolution: programming the geometry of nano-building blocks. J. Am. Chem. Soc. 124, 11244-11245 (2002).
20. Dong, L., Chu, Y., Zuo, Y. & Zhang, W. Two-minute synthesis of PbS nanocubes with high yield and good dispersibility at room temperature. Nanotechnology 20, 125301 (2009).
21. Huang, W.-C., Lyu, L.-M., Yang, Y.-C. & Huang, M. H. Synthesis of Cu2O nanocrystals from cubic to rhombic dodecahedral structures and their comparative photocatalytic activity. J. Am. Chem. Soc. 134, 1261-1267 (2012).
22. Simon, P., et al. Interconnection of nanoparticles within 2D superlattices of PbS/oleic acid thin films. Adv. Mater. 26, 3042-3049 (2014).
23. Boneschanscher, M. P., et al. Long-range orientation and atomic attachment of nanocrystals in 2D honeycomb superlattices. Science 344, 1377-1380 (2014).
24. Matthew, K., Sundararaman, R., Letchworth-Weaver, K., Arias, T. A. & Hennig, R. G. Implicit solvation model for density-functional study of nanocrystal surfaces and reaction pathways. J. Chem. Phys. 140, 084106 (2014).
25. Schapotschnikow, P., van Huis, M. A., Zandbergen, H.W., Vanmaekelberh, D. & Vlugt, T. J. H. Morphological transformations and fusion of PbSe nanocrystals studied using atomistic simulations. Nano Lett. 10, 3966-3971 (2010).
26. Schliehe, C., et al. Ultrathin PbS sheets by two-dimensional oriented attachment. Science 329, 550-2936 (2010).
27. Dirin, N. D., et al. Lead halide perovskites and other metal halide complexes as inorganic capping ligands for colloidal nanocrystals. J. Am. Chem. Soc. 136, 6550-6553 (2014).
28. Ning, Z., et al. Quantum-dot-in-perovskite solids. Nature 523, 324-328 (2015).
29. Li, D., et al. Direction-specific interaction control crystal growth by oriented attachment. Science 336, 1014-1018 (2012).
30. van Huis, M. A., Kunneman, L. T., Overgaag, K., Zandbergen, H.W. & Vanmaekelberh, D. Low-temperature nanocrystal unification through rotations and relaxations probed by in situ transmission electron microscopy. Nano Lett. 10, 3966-3971 (2010).
31. Casavola, M., et al. Anisotropic cation exchange in PbSe/CdSe core/shell nanocrystals of different geometry. Chem. Mater. 8, 3959-3963 (2008).
32. Wuttig, M., et al. The role of vacancies and local distortions in the design of new phase-change materials. Nature Mater. 6, 122-128 (2007).
33. Cervellino, A., et al. Diffuse scattering from the lead-based relaxor ferroelectric PbMg1=3Ta2=3O3. J. Appl. Crystallogr. 44, 603-609 (2011).
34. VandeVondele, J., et al. Quickstep: fast and accurate density functional calculations using a mixed Gaussian and plane waves approach. Comput. Phys. Commun. 167, 103-128 (2005).